As the first unseeded woman in the Wimbledon final in 60 years, Vondrousova was a heavy underdog against sixth-ranked Jabeur.
But the 24-year-old upset the odds on Centre Court to win her maiden Grand Slam title at the second attempt after losing to Ash Barty in the 2019 French Open final.
"After everything I've been through - I had a cast on this time last year - and now I can't believe I'm holding this trophy," said Vondrousova who was sidelined with a wrist injury in 2022.
"I don't know what's happening now."
Vondrousova joins Jana Novotna and Petra Kvitova as the only Czech women to win a Wimbledon title.
She is just the ninth unseeded champion at a Grand Slam tournament.
Vondrousova's triumph completed a remarkable comeback after a rash of injuries stalled her promising career.
Just 12 months ago, she was an injured bystander at Wimbledon, reduced to watching her best friend Miriam Kolodziejova attempt to qualify for the main draw.
Vondrousova's second wrist surgery had ruled the Olympic silver medallist out for six months, although her absence from the tour at least allowed her the space and time to get married.
"The comebacks are not easy. You never know what to expect," she said.
"I was hoping I could come back to this level and now I am here. It's an amazing feeling."
She was the second-lowest ranked player to reach the Wimbledon final -- only Serena Williams in 2018 was lower at 181.
So unexpected was her run that she told her husband Stepan Simek to stay at home in Prague to look after their cat Frankie until the final, when a pet sitter was found to allow her partner to make the trip to Wimbledon.
The defeat was another heartbreaking blow for world number six Jabeur, who wept during an emotional post-match trophy presentation.
Jabeur was the first Arab woman to reach a Grand Slam final last year at Wimbledon, but losing to Elena Rybakina in three sets took the shine off that achievement.
She endured more misery just weeks later when she lost to Iga Swiatek in the US Open final.
"It's going to be a tough day but I am not going to give up," she said while wiping away her tears.
"It's the most painful loss of my career. but we're going to make it one day, I promise you I'm not going to give up."
Ice-cool Vondrousova
Jabeur's bid to become the first African and Arab woman to win a Grand Slam singles title has ended in bitter failure once again.
Even for a player known as the 'Minister of Happiness', Jabeur's positive personality will be tested by her latest disappointment.
She fell well short of the standards shown in victories over four former Grand Slam champions on her way to the final.
Jabeur had already lost twice in 2023 to Vondrousova, at the Australian Open and in Miami, and she had no answer to the big-hitting left-hander despite the support of 15,000 partisan fans on Centre Court.
Under the closed roof, Jabeur drew first blood with a break in the second game when Vondrousova netted a nervous backhand.
But she immediately surrendered the initiative as Vondrousova broke back in the next game.
Jabeur's anxiety was clear as her unforced error total reached double figures in another wild game that gave Vondrousova a 5-4 advantage that she gratefully seized to serve out the set.
Vondrousova made it five games in a row when Jabeur's weak forehand gifted her a break in the opening game of the second set.
Breaking twice in three games, Jabeur moved 3-1 up, only to falter again as the ninth break of the match allowed Vondrousova back into the set.
It was an opportunity the Czech was not going to spurn as Jabeur's unforced errors reached 31 by the final game.
In contrast to Jabeur's meltdown, Vondrousova remained ice-cool and sealed her unexpected triumph with a perfect volley before falling to the turf in delight.
